SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Fanyue Meng,Chenbin Lin,Bing Song,Lei Yu,Yan Zhao,Zejian Zhi,Min Song
This study employed a self-designed underwater arc discharge (UAD) plasma reactor, which combined advanced oxidation process (Fe 2 O 3 -CoFe 2 O 4 /PMS) and low-temperature plasma technology to efficiently degrade refractory organic pollutants (i.e. phenol, p-chlorophenol, p-nitrochlorobenzene). The results illustrated that the plasma/PMS/Fe 2 O 3 -CoFe 2 O 4 system possessed high degradation efficiency and TOC removal rate towards three target pollutants (phenol: 99.8%, 96.12%; 4-CP: 98.4%, 86.48%; p-NCB: 99.9%, 88.31%). With the help of in-situ variable temperature EPR and Indigo colorimetry method, ·OH, SO 4 ·- , O 2 ·- , 1 O 2 and O 3 were identified as the main reactive oxygen species (ROS) for the degradation of target pollutants, revealing the synergistic catalytic mechanism between plasma and Fe 2 O 3 -CoFe 2 O 4 for PMS activation and inferring the degradation pathways of target pollutants. The results confirmed that the plasma/PMS/Fe 2 O 3 -CoFe 2 O 4 system was feasible for the degradation of refractory organic pollutants, has the advantages of high efficiency and low energy consumption, and could provide an effective strategy for the treatment of refractory organic pollutants in groundwater/soil.
研究领域:
环境科学
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化学工程
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水处理
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DOI
高影响因子
ChemistrySelect
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2024
·Vol. 9
·期 8
·e202303088
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IF 1.9
Xiayan Zhang,Zhi Song,Boxia Liu,Jialu Liu,Yeqiong Huang,Dongxu Han
Graphical Ni/Fe bimetallic atom cluster catalyst is prepared by a hydrothermal to stimulate PMS to produce high concentration 1 O 2 and efficiently remove BPA from aqueous solution. It is found that 1 O 2 in the system is the most important active component in the degradation process of BPA, and a high concentration of 1 O 2 could promote the rapid degradation of BPA in solution. The advanced oxidation process based on peroxymonosulfate (PMS) is a new water purification strategy. In this work, Ni/Fe bimetallic atom cluster composite catalyst is prepared by a hydrothermal synthesis to stimulate PMS to produce high concentration singlet oxygen ( 1 O 2 ) and efficiently remove bisphenol A (BPA) from aqueous solution. The experimental data show that in a broad pH range (pH=3–11), the removal rate of BPA by the non-free radical pathway induced by 1 O 2 is close to 100 %, and the catalyst still has high stability after 5 cycles. The mechanism of BPA removal in NiFe−BC/PMS/BPA catalytic degradation system is investigated by quenching experiment. It is found that 1 O 2 in the system is the most important active component in the degradation process of BPA, and a high concentration of 1 O 2 could promote the rapid degradation of BPA in solution. In this paper, the high catalytic activity and selectivity of bimetallic atomic cluster catalysts can provide new insights for the treatment of phenolic wastewater.
研究领域:
环境科学
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催化
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水处理
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化学工程
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Zhilong Zhang,Xingyu Zhan,Bo Hong,Xinqing Wang,Peisong Tang,Yangbin Ding,Yingchun Xia,Yunxiong Zeng
Peroxymonosulfate (PMS) is widely employed to generate oxygen-containing reactive species for ciprofloxacin (CIP) degradation. Herein, cobalt oxyhydroxide @activated carbon (CoOOH@AC) was synthesized via a wet chemical sedimentation method to activate PMS for degradation of CIP. The result suggested AC can support the vertical growth of CoOOH nanosheets to expose high-activity Co-contained edges, possessing efficient PMS activation and degradation activity and catalytic stability. In the presence of 3.0 mg of optimal CoOOH@AC and 2 mM PMS, 96.8 % of CIP was degraded within 10 min, approximately 11.6 and 9.97 times greater than those of CoOOH/PMS and AC/PMS systems. Notably, it was disclosed that the optimal CoOOH@AC/PMS system still exhibited efficient catalytic performance in a wide pH range, different organics and common co-existing ions. Quenching experiments and electron paramagnetic resonance indicated that both radical and non-radical processes contributed to the degradation of CIP, with 1 O 2 and direct electron transfer accounting for the non-radical pathway and SO 4 •− and •OH serving as the main radical active species. Finally, possible CIP degradation pathways were proposed based on high-performance liquid chromatography-mass spectrometry. This study provided an alternate method for wastewater treatment based on PMS catalyzed by cobalt-based hydroxide.
研究领域:
环境科学
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化学工程
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材料科学
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废水处理
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DOI
PubMed
高影响因子
Surfaces and Interfaces
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2025
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IF 6.3
Junxia Chen,Yuying Yang,Weigang Li,Zhenzhen Yang,Yizhou Wu,Yubai Chen,Qing Zhou
The synthesized FeVO 4 /MXene composite photocatalysts demonstrated exceptional photocatalytic activity in activating PMS, removing 100% of 2,4,6-trichlorophenol (2,4,6-TCP) within 20 minutes. The incorporation of MXene effectively reduced photogenerated electron-hole pairs recombination in FeVO₄, enhancing charge transfer efficiency. Mechanistic studies revealed that synthesized FeVO 4 /MXene generated more •OH and ¹O₂ through the reaction between h⁺ and PMS. Furthermore, the photogenerated electrons (e⁻) facilitated Fe redox cycling within the system. The FeVO 4 /MXene/PMS/Vis system not only achieved efficient separation of photogenerated charge carriers but also reduced the required PMS dosage by 75%. Remarkably, the FeVO₄/MXene composite maintained its structural integrity after five consecutive cycles while retaining 98% of its initial degradation efficiency for 2,4,6-TCP, demonstrating excellent durability and promising application potential.
研究领域:
环境科学
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材料科学
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化学工程
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光催化
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DOI
高影响因子
RARE METALS
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2025
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IF 11
Wang Zhenxiao,Ning Shuguang,Liu Xiang,Zhao Hongyao,Zhang Wanyu,Cao Liying,Wang Yanyun,Shang Danhong,Zhai Linzhi,Yang Tongyi,Zeng Feng,Zhang Yangping,Yang Fu
The advanced oxidation process presents a perfect solution for eliminating organic pollutants in water resources, and the local microenvironment and surface state of metal reactive sites are crucial for the selective activation of peroxomonosulfate (PMS), which possibly determines the degradation pathways of organic contaminants. In this study, by virtue of the precursor alternation, we constructed the state-switched dual metal species with the porous carbon fibers through the electrospinning strategy. Impressively, the optimal catalyst, featuring the electron-deficient cobalt surface oxidative state and most abundant oxygen vacancies (Ov) with MnO 2 within porous carbon fibers, provides abundant mesoporosity, facilitating the diffusion and accommodation of big carbamazepine molecules during the reaction process. Benefiting from the tandem configuration of carbon fiber-encapsulated nanocrystalline species, a p–n heterojunction configuration evidenced by Mott–Schottky analysis induced local built-in electric field (BIEF) between electron-deficient cobalt and Ov-rich MnO 2 within carbon matrix-mediated interfacial interactions, which optimizes the adsorption and activation of PMS and intermediates, increases the concentration of reactive radicals around the active site, and significantly enhances the degradation performance. As a result, the optimal catalyst could achieve 100% degradation of 20 ppm carbamazepine (CBZ) within only 4 min with a rate constant of 1.099 min −1 , showcasing a low activation energy (50 kJ mol −1 ), obviously outperforming the other counterparts. We further demonstrated the generation pathways of active species by activation of PMS mainly including sulfate radical (·SO 4 − ), hydroxyl radical (·OH), superoxide radicals (·O 2 − ), and singlet oxygen ( 1 O 2 ), unveiling their contribution to CBZ degradation. The degradation route of CBZ and toxicity analysis of various intermediates were further evaluated. By anchoring the optimal catalyst onto polyester fiber sponge, the photothermal conversion synergistic monolith floatable catalyst and its easy recovery can be achieved, showing good reproducibility and generalizability in the practical application. Graphical abstract
研究领域:
环境科学
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材料科学
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化学工程
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纳米技术
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水处理
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Limeng Yang,Wendou Chen,Cuihong Sheng,Hailiang Wu,Ningtao Mao,Hui Zhang
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are encouraging methods for wastewater treatments, but the recycling of used PMS activators in powder form from the wastewater treatment system is still problematic. In this paper, we designed a novel and highly effective carbocatalyst for PMS activation, which was achieved by pyrolyzing the hybrids of metal–organic framework MIL-101(Fe) and dicyandiamide immobilized on the surface of carbon cloth (CC), and a facile route for the preparation of fibrous catalysts was developed. The resultant CC loaded with Fe/N-codoped carbocatalyst exhibited desirable reusability and good stability for the degradation of organic dyes. The mechanism of the novel Fe/N-codoped carbocatalyst for PMS activation including the specific roles of N species and Fe-N binding was investigated. It was demonstrated in electrochemical impedance spectroscopy (EIS) results that the CC facilitated the electron transport of the carbocatalyst in AOPs. It was shown in the radical quenching and electron paramagnetic resonance (EPR) experiments that both the radical and non-radical pathways were accountable for the degradation of contaminants, and the non-radical path was principal. It was also evident in the X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) results that pyridinic N and graphitic N were the main active species for PMS activation.
研究领域:
环境科学
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催化
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水处理
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Bingyang Liu,Yu Wang,Xue Hao,Xuetao Liang,Qi Yang
In this work, a carbon-based catalyst Fe/Co@C with MOF as a self-sacrificing template was prepared by high-temperature roasting of FeCo-MIL101, which was applied to activate PMS for the degradation of chlorotriazine herbicides (ATZ and SIM) showing excellent performance. Characterization analysis revealed that Fe/Co@C possesses a certain graphene structure and has a saturation magnetization rate of 0.87 emu/g, which can be separated from the solution easily and quickly. The degradation of ATZ and SIM was enhanced by introducing chloride ions into the system, and 100 mmol/L Cl - could lead to the complete removal of ATZ and SIM in 6 min, while improving the interfacial electron transfer of Fe/Co@C/PMS. In combination with quenching experiments, ESR test results and DFT calculations, two important roles of chlorine radicals in the reaction are proposed: (1) direct electron transfer and (2) indirect promotion of 1 O 2 generation through the production of HOCl. In addition, the testing of the influencing factors of the catalyst in the system (catalyst dosing, PMS dosing, pH, temperature), the testing of coexisting anions in the aqueous matrix, and the reusability all showed satisfactory performance. Finally, the degradation mechanisms of ATZ and SIM were proposed in combination with GC–MS determination of contaminant intermediates and analysis of their toxicity.
研究领域:
环境科学
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催化
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水处理
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化学工程
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DOI
高影响因子
Environmental Science-Nano
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2020
·Vol. 7
·期 10
·2982-2994
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IF 7.683
Weijian Duan,Jinglei He,Ziliang Wei,Zongren Dai,Chunhua Feng
The heteroatom-doped, carbon-activated peroxymonosulfate (PMS) system proceeding via the non-radical oxidation pathway involving singlet oxygen (1O2) represents a promising advanced oxidation process (AOP) due to the resistance of 1O2 to background anions in solution. However, the performance level of pollutant removal is not yet satisfied, and the mechanism of 1O2 generation remains elusive. Herein, we report the development for the first time of a unique Si-engaged heteroatom (i.e., N)-doped carbon (Si/N–C) nanomaterial for PMS activation, which exhibits outstanding performance in the removal of various kinds of pollutants and an appreciably wide working pH range of 2.5 to 11. Taking rhodamine B (RhB) as an example, the Si/N–C@PMS system achieved a much higher reaction rate (0.64 min−1) than the Si–C (0.047 min−1), N–C (0.017 min−1), SiO2 (0.021 min−1), and Co3O4 (0.026 min−1; a standard catalyst) systems. In addition, the results of electron spin resonance (ESR) and scavenging experiments solidly support the conclusion that the mechanism of 1O2 generation in this system is via the recombination of superoxide radicals O2˙−, a pathway seldom reported for metal-free, catalyst-activated PMS systems. More importantly, we observed apparent inhibition effects of the anions (e.g., HCO3−, HPO42−, and PO43−) on the degradation performance, inconsistent with many previous reports suggesting that the 1O2-mediated oxidative system possesses a high selectivity toward pollutant degradation in the presence of these anions. Further studies with the anions, including Cl−, HCO3−, and HxPO4(3−x) (x = 0, 1, 2), suggest that the reaction between O2˙− and these anions is the main reason for the abnormal salt effect. This work will deepen the understanding of 1O2 formation via the intermediate of O2˙− and provide a new insight into its salt resistance capacity.
研究领域:
环境化学
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材料科学
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催化
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水处理
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jing Wang,Ziyang Chu,Haibo Liu,Zhengyan Han,Tianhu Chen,Xuehua Zou,Dong Chen
Advanced oxidation processes employing natural carbonate minerals to activate peroxymonosulfate (PMS) have exhibited remarkable efficacy in the removal of organic pollutants. In this study, the differences in the degradation performance and mechanism of chloroquine phosphate (CQP) by calcite/PMS and dolomite/PMS systems were investigated. Experimental findings reveal that the calcite/PMS system demonstrates markedly superior removal under identical conditions, achieving 99 % CQP removal within 60 min. In contrast, the dolomite/PMS system only achieved 63 % CQP removal under the same conditions. Electron paramagnetic resonance (EPR) and radical quenching analyses identified singlet oxygen ( 1 O 2 ) as the dominant reactive species in both systems. Quantitative assessments indicated that the calcite/PMS system generated more 1 O 2 (43.3 μM) compared to the dolomite/PMS system (35.4 μM.). This phenomenon was attributed to that calcite released more carbonate ions (CO 3 2− ) than dolomite. Although the two systems had different reaction rates, both achieved stable CQP removal over 90 % in a one-month continuous flow column experiments. This work developed the application potential of carbonate minerals in advanced oxidation systems. Furthermore, the findings contribute to better understanding and development of carbonate activated persulfate systems.
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高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Xinyu Liu,Jianlong Wang
The efficient elimination of ammonia nitrogen (NH 4 + -N) from the specific wastewater and selective oxidation to nitrogen gas are the most desirable purposes of wastewater treatment, but still remains a challenge. Herein, we presented a cobalt-based catalyst (Co-VB 12 -C) as a novel heterogeneous catalyst, which was fabricated via the co-pyrolysis of poly (2,6-diaminopyridine) and vitamin B 12 . Co-VB 12 -C were successfully prepared to construct a facile heterogeneous Co-VB 12 -C/PMS/Cl system and achieve effective removal of NH 4 + -N and high selectivity to nitrogen gas in acidic and neutral pH. Co-VB 12 -C had superior catalytic capability, reusability, and stability. The role of catalyst, PMS, Cl - , and pH value was investigated and the corresponding mechanism was proposed, which revealed that Cl•-mediated oxidation reactions made predominant contribution to NH 4 + -N transformation. This system is a facile alternative technology for removing ammonium from high saline wastewater.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Journal of Environmental Sciences
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2020
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IF 4.302
Xiaoyang Fan,Yili Wang,Daxin Zhang,Yajie Guo,Shihui Gao,Enrui Li,Huaili Zheng
The effects of four conditioning approaches: Acid, Acid-zero-valent iron (ZVI)/peroxydisulfate (PMS), Fe(II)/PMS and ZVI/PMS, on wastewater activated sludge (WAS) dewatering and organics distribution in supernatant and extracellular polymeric substances (EPS) layers were investigated. The highest reduction in bound water and the most WAS destruction was achieved by Acid-ZVI/PMS, and the optimum conditions were pH 3, ZVI dosage 0.15 g/g dry solid (DS), oxone dosage 0.07 g/g DS and reaction time 10.6 min with the reductions in capillary suction time (CST) and water content (Wc) as 19.67% and 8.49%, respectively. Four conditioning approaches could result in TOC increase in EPS layers and supernatant, and protein (PN) content in tightly bound EPS (TB-EPS). After conditioning, organics in EPS layers could migrate to supernatant. Polysaccharide (PS) was easier to migrate to supernatant than PN. In addition, Acid, Acid-ZVI/PMS or Fe(II)/PMS conditioning promoted the release of some polysaccharides containing ring vibrations v P O, v C-O-C, v C-O-P functional groups from TB-EPS. ESR spectra proved that both radicals of SO 4 - · and ·OH contributed to dewatering and organics transformation and migration. CST value of WAS positively correlated with the ratios of PN/PS in LB-EPS and total EPS, while it negatively correlated with TOC, PN content and PS content in TB-EPS, as well as PS content in supernatant and LB-EPS. BWC negatively correlated to zeta potential and TOC value, PN content, and HA content in supernatant.
研究领域:
环境科学
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污水处理
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
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2020
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IF 5.778
Haopeng Luo,Xin Zhou,Xiaojie Guo,Zhiyong Fang,Quanyuan Chen,Juan Zhou
The greatest constraint in the advanced oxidation processes involved Fe(II)/PMS was the low utilization of Fe(II) and PMS. In the present study, the co-catalytic effect of WS 2 on the Fe(II)/PMS system for the degradation of organics was investigated. In the presence of WS 2 , Fe(III) was reduced to Fe(II) during the reaction and resulted in improved decomposition of PMS as well as the degradation of 4-chloriphenol (4-CP). The decomposition rate of PMS and degradation efficiency of 4-CP were 10% and 25% in the Fe(II)/PMS process, while the efficiencies respectively increased to 99% and 100% in the WS 2 assisted Fe(II)/PMS system. The degradation of 4-CP was completed via the free radical pathway and SO 4 • - played a more important role than other active species. Low concentration of inorganic ions such as Cl − and HCO 3 − exhibited irrelevant effect while humic acid showed significant suppression on the WS 2 /Fe(II)/PMS system. Additionally, characterization and recycle results implied that WS 2 maintained a good stability during the co-catalytic processes.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
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